Assembly and disassembly of proteins, nature's macromolecules, in response to a specific stimulus is ubiquitous in biology. Mimicking these processes, where proteins are used as the stimulus to disassemble artificial macromolecular assemblies are interesting for a variety of biomedical applications. For example, although targeted drug delivery is not a specific goal for this proposal, the experiments proposed here to obtain the proof-of-concept could have a significant impact in this area. Specifically, this proposal describes the development of versatile strategies to disassemble dendrimer-based amphiphilic assemblies using proteins as stimuli. Facially amphiphilic dendrimers, reported by us recently in the literature, are a unique class of molecules in that these are the only class of amphiphilic dendrimers that form micelle-type assemblies through aggregation. Even more interesting is the fact that these assemblies can be disassembled in response to a stimulus. While stimuli-responsive assemblies themselves have been studied quite extensively, reports where proteins are used as the stimulus for disassembling organized supramolecular assemblies are rather limited. This proposal describes a concerted approach to this problem, which could have broad implications in biology and medicine.